The characteristics and mechanism of NO formation during pyridine oxidation in O2/N2 and O2/CO2 atmospheres
The characteristics and mechanism of NO formation during pyridine oxidation in O2/N2 and O2/CO2 atmospheres
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O2/N2和O2/CO2气氛中吡啶氧化过程中NO生成的特征和机理
DOI：
10.1016/j.energy.2019.115954
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发表时间：
2019-11
期刊：
影响因子：
9
通讯作者：
Sizhe Cheng
中科院分区：
文献类型：
--
作者：
Jianghui Luo;Chun Zou （通讯作者）;Yizhuo He;Huixiang Jing;Sizhe Cheng
从实验和数值两个方面研究了O2/CO2气氛中吡啶氧化过程中NO生成的特征和机理。在常压流动反应器中，在773 K~1573 K温度范围内进行了O2/N_2和O_2/CO_2两种气氛下的对比实验。实验结果表明，HCN在CO_2气氛中完全消耗，而在富燃料条件下大量残留在N_2气氛中。与O2/N2气氛相比，在化学计量比和贫油条件下，O2/CO2气氛中NO的生成量分别减少了8.85%和5.8%，而在富燃料条件下则增加了5.15%。在前人研究的基础上，新发展的化学动力学机制令人满意地再现了CO、HCN和NO生成的主要特征。在O2/CO2和O2/N2气氛中，吡啶转化为NO的差异主要是由于HCN转化为NO的差异所致。吡啶对HCN的转化率偏差均小于2%。在富燃料条件下，O2/N2和O2/CO2气氛中HCN到NO的转化率分别为7.2%和15.6%，化学计量比条件下分别为65.3%和57.4%，贫油条件下分别为83.5%和76.3%。
The characteristics and mechanism of NO formation during pyridine oxidation in O2/CO2atmospheres are investigated both experimentally and numerically. Comparison experiments in O2/N2and O2/CO2atmospheres are performed in a flow reactor at atmospheric pressure covering fuel-rich to fuel-lean equivalence ratios with temperature ranging from 773 K to 1573 K. Experimental results indicated that HCN is completely consumed in CO2atmospheres, whereas significant amounts remain in N2atmospheres under fuel-rich conditions. Compared with O2/N2atmospheres, the formation of NO in O2/CO2atmospheres is reduced by 8.85% and 5.8% under stoichiometric and fuel-lean conditions respectively, whereas it is 5.15% greater under fuel-rich conditions. A newly developed chemical kinetic mechanism based on our previous studies satisfactorily reproduced the main features of CO, HCN, and NO formation. The conversion differences of pyridine to NO between O2/CO2and O2/N2atmospheres are mainly due to the differences of conversion of HCN to NO. The conversion ratio discrepancies of pyridine to HCN are all less than 2%. The conversion ratios of HCN to NO in O2/N2and O2/CO2atmospheres are 7.2% and 15.6% under fuel-rich conditions, 65.3% and 57.4% under stoichiometric conditions, and 83.5% and 76.3% under fuel-lean conditions, respectively.
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